Probing the Origin of Chiral Charge Density Waves in the Two-Dimensional Limits

Chirality generates spontaneous symmetry breaking and profoundly influences the topology, charge, and spin orders of materials. The chiral charge density wave (CDW) exhibits macroscopic chirality in the achiral crystal during the spontaneous electronic phase transitions. However, the mechanism of chiral CDW formation is shrouded in controversy. In this work, we report that two-dimensional H-phase TaS2 synthesized by molecular-beam epitaxy (MBE) shows a predominantly chiral CDW phase. Scanning tunneling microscopy (STM) imaging of the CDW reconstruction spots reveals a clockwise or anticlockwise intensity variation along the STM-imaged spots. First-principles calculations further show that the rotational symmetry of the momentum-dependent electronphonon coupling is broken, giving rise to chirality. Our work provides new insights into the physical origin of the chiral charge-ordered states, shedding light on a general ordering rule in chiral CDWs.